Declining calcium concentration drives shifts toward smaller and less nutritious zooplankton in northern lakes.

Zooplankton community composition of northern lakes is changing due to the interactive effects of climate change and recovery from acidification, yet limited data are available to assess these changes combined. Here, we built a database using archives of temperature, water chemistry and zooplankton data from 60 Scandinavian lakes that represent broad spatial and temporal gradients in key parameters: temperature, calcium (Ca), total phosphorus (TP), total organic carbon (TOC), and pH. Using machine learning techniques, we found that Ca was the most important determinant of the relative abundance of all zooplankton groups studied, while pH was second, and TOC third in importance. Further, we found that Ca is declining in almost all lakes, and we detected a critical Ca threshold in lake water of 1.3 mg L-1 , below which the relative abundance of zooplankton shifts toward dominance of Holopedium gibberum and small cladocerans at the expense of Daphnia and copepods. Our findings suggest that low Ca concentrations may shape zooplankton communities, and that current trajectories of Ca decline could promote widespread changes in pelagic food webs as zooplankton are important trophic links from phytoplankton to fish and different zooplankton species play different roles in this context.

Long-term rise in riverine dissolved organic carbon concentration is predicted by electrolyte solubility theory.

The riverine dissolved organic carbon (DOC) flux is of similar magnitude to the terrestrial sink for atmospheric CO2, but the factors controlling it remain poorly determined and are largely absent from Earth system models (ESMs). Here, we show, for a range of European headwater catchments, that electrolyte solubility theory explains how declining precipitation ionic strength (IS) has increased the dissolution of thermally moderated pools of soluble soil organic matter (OM), while hydrological conditions govern the proportion of this OM entering the aquatic system. Solubility will continue to rise exponentially with declining IS until pollutant ion deposition fully flattens out under clean air policies. Future DOC export will increasingly depend on rates of warming and any directional changes to the intensity and seasonality of precipitation and marine ion deposition. Our findings provide a firm foundation for incorporating the processes dominating change in this component of the global carbon cycle in ESMs.

Assessing critical load exceedances and ecosystem impacts of anthropogenic nitrogen and sulphur deposition at unmanaged forested catchments in Europe.

Anthropogenic emissions of nitrogen (N) and sulphur (S) compounds and their long-range transport have caused widespread negative impacts on different ecosystems. Critical loads (CLs) are deposition thresholds used to describe the sensitivity of ecosystems to atmospheric deposition. The CL methodology has been a key science-based tool for assessing the environmental consequences of air pollution. We computed CLs for eutrophication and acidification using a European long-term dataset of intensively studied forested ecosystem sites (n = 17) in northern and central Europe. The sites belong to the ICP IM and eLTER networks. The link between the site-specific calculations and time-series of CL exceedances and measured site data was evaluated using long-term measurements (1990-2017) for bulk deposition, throughfall and runoff water chemistry. Novel techniques for presenting exceedances of CLs and their temporal development were also developed. Concentrations and fluxes of sulphate, total inorganic nitrogen (TIN) and acidity in deposition substantially decreased at the sites. Decreases in S deposition resulted in statistically significant decreased concentrations and fluxes of sulphate in runoff and decreasing trends of TIN in runoff were more common than increasing trends. The temporal developments of the exceedance of the CLs indicated the more effective reductions of S deposition compared to N at the sites. There was a relation between calculated exceedance of the CLs and measured runoff water concentrations and fluxes, and most sites with higher CL exceedances showed larger decreases in both TIN and H+ concentrations and fluxes. Sites with higher cumulative exceedance of eutrophication CLs (averaged over 3 and 30 years) generally showed higher TIN concentrations in runoff. The results provided evidence on the link between CL exceedances and empirical impacts, increasing confidence in the methodology used for the European-scale CL calculations. The results also confirm that emission abatement actions are having their intended effects on CL exceedances and ecosystem impacts.

Cleaner air reveals growing influence of climate on dissolved organic carbon trends in northern headwaters.

Surface water browning, the result of increasing concentrations of dissolved organic matter (DOM), has been widespread in northern ecosystems in recent decades. Here, we assess a database of 426 undisturbed headwater lakes and streams in Europe and North America for evidence of trends in DOM between 1990 and 2016. We describe contrasting changes in DOM trends in Europe (decelerating) and North America (accelerating), which are consistent with organic matter solubility responses to declines in sulfate deposition. While earlier trends (1990-2004) were almost entirely related to changes in atmospheric chemistry, climatic and chemical drivers were equally important in explaining recent DOM trends (2002-2016). We estimate that riverine DOM export from northern ecosystems increased by 27% during the study period. Increased summer precipitation strengthened upward dissolved organic carbon trends while warming apparently damped browning. Our results suggest strong but changing influences of air quality and climate on the terrestrial carbon cycle, and on the magnitude of carbon export from land to water.

Streamwater responses to reduced nitrogen deposition at four small upland catchments in Norway.

Reduced emissions of nitrogen (N) in Europe have resulted in decreasing atmospheric deposition since 1990. Long-term data (1988-2017) from four small Norwegian catchments located along gradients in N deposition, rainfall, and organic carbon (C) show different responses to 25-30% reductions in N deposition during the same period. At three sites the decreased N deposition caused reduced leaching of nitrate to surface water, whereas the westernmost site showed no decrease, probably due to thin soils with low C:N ratio, poor vegetation cover and high precipitation. The loss of total N to streamwater constituted 30-50% of the N deposition. Losses via denitrification are unknown but assumed to be low, as a major fraction of the catchments are well-drained. Hence, the study sites seem to continue to accumulate N, presumably mostly in soil organic matter. Although atmospheric N deposition has declined, ambient loads might still exceed long-term sustainable levels in these vulnerable ecosystems.

Recent advances in understanding and measurement of mercury in the environment: Terrestrial Hg cycling.

This review documents recent advances in terrestrial mercury cycling. Terrestrial mercury (Hg) research has matured in some areas, and is developing rapidly in others. We summarize the state of the science circa 2010 as a starting point, and then present the advances during the last decade in three areas: land use, sulfate deposition, and climate change. The advances are presented in the framework of three Hg "gateways" to the terrestrial environment: inputs from the atmosphere, uptake in food, and runoff with surface water. Among the most notable advances: These and other advances reported here are of value in evaluating the effectiveness of the Minamata Convention on reducing environmental Hg exposure to humans and wildlife.

Five decades of declining methylmercury concentrations in boreal foodwebs suggest pivotal role for sulphate deposition.

Widespread declines in mercury (Hg) in fish in pristine lakes in Fennoscandia since the 1970s are unexplained. Interactions between climate, atmospheric deposition, and elemental cycling of carbon (C), sulphur (S) and Hg are complex and affect Hg bioaccumulation. A parallel significant decline in methyl-Hg (MeHg) concentrations in aquatic macroinvertebrates (Chironomidae) was found between 1976-78 and 2004-15 in an intensely studied, pristine boreal lake (Langtjern, boreal Fennoscandia). Monitoring at Langtjern demonstrated a four-fold decrease in aqueous sulphate concentrations (SO4, 50-year record), significant lake browning (30-year records), increasing sediment Hg concentrations (50-year record), warming (45-year record) and increased runoff (40-year record). Contrasting Hg trends in biota (downward) and sediment (upward) indicated a disconnect between lake Hg loading and foodweb Hg bioaccumulation. We suggest that reduced SO4-deposition has 1) constrained substrate availability for SO4-reducing methylating bacteria (causing reduced foodweb MeHg exposure despite increased Hg loading to the lake), and 2), increased the binding affinity between aqueous organic matter and Hg species (leading to reduced MeHg bioavailability). The downward MeHg trend at the base of the foodweb at Langtjern is mirrored at higher trophic levels by strong declines in perch (Perca fluviatilis) and pike (Esox lucius) Hg concentrations in boreal Fennoscandia. A plausible explanation is that declining SO4-deposition, rather than climate change or reduced atmospheric Hg, is currently driving reduced MeHg contamination in northern freshwater foodwebs.

Widespread diminishing anthropogenic effects on calcium in freshwaters.

Calcium (Ca) is an essential element for almost all living organisms. Here, we examined global variation and controls of freshwater Ca concentrations, using 440 599 water samples from 43 184 inland water sites in 57 countries. We found that the global median Ca concentration was 4.0 mg L-1 with 20.7% of the water samples showing Ca concentrations ≤ 1.5 mg L-1, a threshold considered critical for the survival of many Ca-demanding organisms. Spatially, freshwater Ca concentrations were strongly and proportionally linked to carbonate alkalinity, with the highest Ca and carbonate alkalinity in waters with a pH around 8.0 and decreasing in concentrations towards lower pH. However, on a temporal scale, by analyzing decadal trends in >200 water bodies since the 1980s, we observed a frequent decoupling between carbonate alkalinity and Ca concentrations, which we attributed mainly to the influence of anthropogenic acid deposition. As acid deposition has been ameliorated, in many freshwaters carbonate alkalinity concentrations have increased or remained constant, while Ca concentrations have rapidly declined towards or even below pre-industrial conditions as a consequence of recovery from anthropogenic acidification. Thus, a paradoxical outcome of the successful remediation of acid deposition is a globally widespread freshwater Ca concentration decline towards critically low levels for many aquatic organisms.

Improved Environmental Status: 50 Years of Declining Fish Mercury Levels in Boreal and Subarctic Fennoscandia.

Temporally (1965-2015) and spatially (55°-70°N) extensive records of total mercury (Hg) in freshwater fish showed consistent declines in boreal and subarctic Fennoscandia. The database contains 54 560 fish entries ( n: pike > perch ≫ brown trout > roach ≈ Arctic charr) from 3132 lakes across Sweden, Finland, Norway, and Russian Murmansk area. 74% of the lakes did not meet the 0.5 ppm limit to protect human health. However, after 2000 only 25% of the lakes exceeded this level, indicating improved environmental status. In lakes where local pollution sources were identified, pike and perch Hg concentrations were significantly higher between 1965 and 1990 compared to values after 1995, likely an effect of implemented reduction measures. In lakes where Hg originated from long-range transboundary air pollution (LRTAP), consistent Hg declines (3-7‰ per year) were found for perch and pike in both boreal and subarctic Fennoscandia, suggesting common environmental controls. Hg in perch and pike in LRTAP lakes showed minimal declines with latitude, suggesting that drivers affected by temperature, such as growth dilution, counteracted Hg loading and food web exposure. We recommend that future fish Hg monitoring sampling design should include repeated sampling and collection of pollution history, water chemistry, fish age, and stable isotopes to enable evaluation of emission reduction policies.

Long-term changes (1990-2015) in the atmospheric deposition and runoff water chemistry of sulphate, inorganic nitrogen and acidity for forested catchments in Europe in relation to changes in emissions and hydrometeorological conditions.

The international Long-Term Ecological Research Network (ILTER) encompasses hundreds of long-term research/monitoring sites located in a wide array of ecosystems that can help us understand environmental change across the globe. We evaluated long-term trends (1990-2015) for bulk deposition, throughfall and runoff water chemistry and fluxes, and climatic variables in 25 forested catchments in Europe belonging to the UNECE International Cooperative Programme on Integrated Monitoring of Air Pollution Effects on Ecosystems (ICP IM). Many of the IM sites form part of the monitoring infrastructures of this larger ILTER network. Trends were evaluated for monthly concentrations of non-marine (anthropogenic fraction, denoted as x) sulphate (xSO4) and base cations x(Ca+Mg), hydrogen ion (H+), inorganic N (NO3 and NH4) and ANC (Acid Neutralising Capacity) and their respective fluxes into and out of the catchments and for monthly precipitation, runoff and air temperature. A significant decrease of xSO4 deposition resulted in decreases in concentrations and fluxes of xSO4 in runoff, being significant at 90% and 60% of the sites, respectively. Bulk deposition of NO3 and NH4 decreased significantly at 60-80% (concentrations) and 40-60% (fluxes) of the sites. Concentrations and fluxes of NO3 in runoff decreased at 73% and 63% of the sites, respectively, and NO3 concentrations decreased significantly at 50% of the sites. Thus, the LTER/ICP IM network confirms the positive effects of the emission reductions in Europe. Air temperature increased significantly at 61% of the sites, while trends for precipitation and runoff were rarely significant. The site-specific variation of xSO4 concentrations in runoff was most strongly explained by deposition. Climatic variables and deposition explained the variation of inorganic N concentrations in runoff at single sites poorly, and as yet there are no clear signs of a consistent deposition-driven or climate-driven increase in inorganic N exports in the catchments.

Mercury in fish from Norwegian lakes: The complex influence of aqueous organic carbon.

Mercury (Hg) concentrations in water and biota are often positively correlated to organic matter (OM), typically measured as total or dissolved organic carbon (TOC/DOC). However, recent evidence suggests that higher OM concentrations inhibit bioaccumulation of Hg. Here, we test how TOC impacts the Hg accumulation in fish in a synoptic study of Methyl-Hg (MeHg) in water and total Hg (THg) in perch (Perca fluviatilis) in 34 boreal lakes in southern Norway. We found that aqueous MeHg (r2 = 0.49, p < 0.0001) and THg (r2 = 0.69, p < 0.0001), and fish THg (r2 = 0.26, p < 0.01) were all positively related with TOC. However, we found declining MeHg bioaccumulation factors (BAFMeHg) for fish with increasing TOC concentrations. The significant correlation between fish THg concentrations and aqueous TOC suggests that elevated fish Hg levels in boreal regions are associated with humic lakes. The declining BAFMeHg with increasing TOC suggest that increased OM promotes increased aqueous Hg concentrations, but lowers relative MeHg bioaccumulation. A mechanistic understanding of the response from OM on BAFMeHg might be found in the metal-complexation properties of OM, where OM complexation of metals reduces their bioavailability. Hence, suggesting that MeHg bioaccumulation becomes less effective at higher TOC, which is particularly relevant when assessing potential responses of fish Hg to predicted future changes in OM inputs to boreal ecosystems. Increased browning of waters may affect fish Hg in opposite directions: an increase of food web exposure to aqueous Hg, and reduced bioavailability of Hg species. However, the negative relationship between BAFMeHg and TOC is challenging to interpret, and carries a great deal of uncertainty, since this relationship may be driven by the underlying correlation between TOC and MeHg (i.e. spurious correlations). Our results suggest that the trade-off between Hg exposure and accumulation will have important implications for the effects of lake browning on Hg transport, bioavailability, and trophodynamics.

Effects of disturbance and vegetation type on total and methylmercury in boreal peatland and forest soils.

Mercury (Hg) concentrations in freshwater fish relates to aquatic Hg concentrations, which largely derives from soil stores of accumulated atmospheric deposition. Hg in catchment soils as a source for aquatic Hg is poorly studied. Here we test if i) peatland soils produce more methylmercury (MeHg) than forest soils; ii) total Hg (THg) concentrations in top soils are determined by atmospheric inputs, while MeHg is produced in the soils; and iii) soil disturbance promotes MeHg production. In two small boreal catchments, previously used in a paired-catchment forest harvest manipulation study, forest soils and peatlands were sampled and analysed for Hg species and additional soil chemistry. In the undisturbed reference catchment, soils were sampled in different vegetation types, of varying productivity as reflected in tree density, where historical data on precipitation and throughfall Hg and MeHg fluxes were available. Upper soil THg contents were significantly correlated to throughfall inputs of Hg, i.e. lowest in the tree-less peatland and highest in the dense spruce forest. For MeHg, top layer concentrations were similar in forest soils and peatlands, likely related to atmospheric input and local production, respectively. The local peatland MeHg production was documented through significantly higher MeHg-to-THg ratios in the deeper soil layer samples. In the disturbed catchment, soils were sampled in and just outside wheeltracks in an area impacted by forest machinery. Here, MeHg concentrations and the MeHg-to-THg ratios in the upper 5 cm were weakly significantly (p = 0.07) and significantly (p = 0.04) different in and outside of the wheeltracks, respectively, suggesting that soil disturbance promotes methylation. Differences in catchment Hg and MeHg streamwater concentrations were not explained by soil Hg and MeHg information, perhaps because hydrological pathways are a stronger determinant of streamwater chemistry than small variations in soil chemistry driven by disturbance and atmospheric inputs of Hg.

From greening to browning: Catchment vegetation development and reduced S-deposition promote organic carbon load on decadal time scales in Nordic lakes.

Increased concentrations of dissolved organic carbon (DOC), often labelled "browning", is a current trend in northern, particularly boreal, freshwaters. The browning has been attributed to the recent reduction in sulphate (S) deposition during the last 2 to 3 decades. Over the last century, climate and land use change have also caused an increasing trend in vegetation cover ("greening"), and this terrestrially fixed carbon represents another potential source for export of organic carbon to lakes and rivers. The impact of this greening on the observed browning of lakes and rivers on decadal time scales remains poorly investigated, however. Here, we explore time-series both on water chemistry and catchment vegetation cover (using NDVI as proxy) from 70 Norwegian lakes and catchments over a 30-year period. We show that the increase in terrestrial vegetation as well as temperature and runoff significantly adds to the reduced SO4-deposition as a driver of freshwater DOC concentration. Over extended periods (centuries), climate mediated changes in vegetation cover may cause major browning of northern surface waters, with severe impact on ecosystem productivity and functioning.

Effects of photodemethylation on the methylmercury budget of boreal Norwegian lakes.

Methylmercury (MeHg) concentrations in freshwater fish from southeastern Norway continue to increase, highlighting the need for a comprehensive understanding of MeHg sources, cycling, and degradation in the aquatic environment. The authors assessed the importance of photodemethylation in the MeHg budget of 4 Norwegian lakes. Photodemethylation rates were determined using incubation experiments with MeHg-spiked natural lake water. The authors determined full-spectrum exposure rates at all study sites and waveband-specific rates (photosynthetically active radiation, ultraviolet-A radiation, and ultraviolet-B radiation) at 1 clear-water (Sognsvann) and 1 humic (Langtjern) site. No significant differences in photodemethylation rates between the sites were found, and the authors' observed rates agreed with available literature for lake and wetland waters. The authors paired experimentally derived photodemethylation rates with lake-specific incident irradiation, light attenuation, and MeHg concentrations to estimate MeHg loss through photodemethylation for the study sites. For Langtjern, losses through photodemethylation equalled 27% of total annual inputs, highlighting the importance of photodemethylation in the MeHg budget. Furthermore, the authors assessed how changes in terrestrial dissolved organic carbon (DOC) exported to freshwaters and climate-driven reductions in ice cover duration may affect MeHg losses through photodemethylation. Results suggest that future increases in DOC may lead to higher aqueous MeHg concentrations in boreal lakes due to increased DOC-associated MeHg inputs paired with significant decreases in the loss of MeHg through photodemethylation due to increased light attenuation.

Environmental factors influencing mercury speciation in Subarctic and Boreal lakes.

Environmental drivers of total mercury (TotHg) concentrations, methylmercury (MeHg) concentrations, and MeHg fractions (a proxy for methylation potential, expressed as %MeHg) were assessed in a synoptic study of 51 lakes in southeast (Boreal) and northeast (Subarctic) Norway. Concentrations of TotHg and MeHg ranged between 0.5-6.6 ng/L and <0.02-0.70 ng/L, respectively. The lakes span wide ranges of explanatory environmental variables, including water chemistry, catchment characteristics, climate conditions, and atmospheric deposition of Hg, sulphur and nitrogen (N). Dissolved organic matter (DOM), measured as total organic carbon (TOC), was the variable most strongly correlated with TotHg (r(2)=0.76) and MeHg (r(2)=0.64) concentrations. Lakes in the Subarctic region had significantly lower TotHg and MeHg concentrations, and %MeHg than lakes in the Boreal region (p<0.01), implying a lower aquatic food web exposure of aqueous Hg species in Subarctic Norway than in the Boreal lakes. Statistical modelling (partial least squares) using data from the Boreal lakes produced models explaining 82%, 75% and 50% of the spatial variation of TotHg and MeHg concentrations and %MeHg, respectively. After TOC, the most significant explanatory variables were N availability, base cation status, and lake and catchment size. We conclude that a key process driving TotHg concentrations is DOM as a transport vector, while the role of DOM for MeHg and %MeHg is likely related to a combination of transport and DOM as a substrate for methylation. Also, negative correlations between MeHg, and catchment and lake size are consistent with in-lake and in-stream de-methylation processes. The statistical relationship suggests that N availability exerts a positive contribution on concentrations of MeHg and %MeHg.

Climate warming feedback from mountain birch forest expansion: reduced albedo dominates carbon uptake.

Expanding high-elevation and high-latitude forest has contrasting climate feedbacks through carbon sequestration (cooling) and reduced surface reflectance (warming), which are yet poorly quantified. Here, we present an empirically based projection of mountain birch forest expansion in south-central Norway under climate change and absence of land use. Climate effects of carbon sequestration and albedo change are compared using four emission metrics. Forest expansion was modeled for a projected 2.6 °C increase in summer temperature in 2100, with associated reduced snow cover. We find that the current (year 2000) forest line of the region is circa 100 m lower than its climatic potential due to land-use history. In the future scenarios, forest cover increased from 12% to 27% between 2000 and 2100, resulting in a 59% increase in biomass carbon storage and an albedo change from 0.46 to 0.30. Forest expansion in 2100 was behind its climatic potential, forest migration rates being the primary limiting factor. In 2100, the warming caused by lower albedo from expanding forest was 10 to 17 times stronger than the cooling effect from carbon sequestration for all emission metrics considered. Reduced snow cover further exacerbated the net warming feedback. The warming effect is considerably stronger than previously reported for boreal forest cover, because of the typically low biomass density in mountain forests and the large changes in albedo of snow-covered tundra areas. The positive climate feedback of high-latitude and high-elevation expanding forests with seasonal snow cover exceeds those of afforestation at lower elevation, and calls for further attention of both modelers and empiricists. The inclusion and upscaling of these climate feedbacks from mountain forests into global models is warranted to assess the potential global impacts.

Methylmercury bioaccumulation in invertebrates of boreal streams in Norway: effects of aqueous methylmercury and diet retention.

Transfer of aqueous methylmercury (MeHg) to primary consumers in aquatic foodwebs is poorly understood despite its importance for bioaccumulation of MeHg. We studied bioaccumulation of MeHg in simple aquatic food chains of two humic boreal streams in relation to streamwater chemistry, food web characteristics and dietary fatty acid (FA) biomarkers. Transfer of aqueous MeHg into primary consumers was similar in both streams, resulting in higher MeHg in consumers in the MeHg-rich stream. Trophic enrichment of MeHg and dietary retention of FA biomarkers was the same in both streams, suggesting that exposure to aqueous MeHg at the base of the food chain determined levels of MeHg in biota. In addition, contents of dietary biomarkers suggested that ingestion of algae reduced MeHg bioaccumulation, while ingestion of bacteria stimulated MeHg uptake. Dietary uptake of bacteria could thus be an important pathway for MeHg-transfer at the bottom of food chains in humic streams.

Testing seasonal and long-term controls of streamwater DOC using empirical and process-based models.

Concentrations of dissolved organic carbon (DOC) in surface waters are increasing across Europe and parts of North America. Several mechanisms have been proposed to explain these increases including reductions in acid deposition, change in frequency of winter storms and changes in temperature and precipitation patterns. We used two modelling approaches to identify the mechanisms responsible for changing surface water DOC concentrations. Empirical regression analysis and INCA-C, a process-based model of stream-water DOC, were used to simulate long-term (1986--2003) patterns in stream water DOC concentrations in a small boreal stream. Both modelling approaches successfully simulated seasonal and inter-annual patterns in DOC concentration. In both models, seasonal patterns of DOC concentration were controlled by hydrology and inter-annual patterns were explained by climatic variation. There was a non-linear relationship between warmer summer temperatures and INCA-C predicted DOC. Only the empirical model was able to satisfactorily simulate the observed long-term increase in DOC. The observed long-term trends in DOC are likely to be driven by in-soil processes controlled by SO4(2-) and Cl(-) deposition, and to a lesser extent by temperature-controlled processes. Given the projected changes in climate and deposition, future modelling and experimental research should focus on the possible effects of soil temperature and moisture on organic carbon production, sorption and desorption rates, and chemical controls on organic matter solubility.

Mercury budget of a small forested boreal catchment in southeast Norway.

We present input and output fluxes of total mercury (Hg(tot)) and methyl mercury (MeHg) based on throughfall, litterfall and stream water samples from 2004/2005 from a small forested catchment (Langtjern) in Norway. Hg(tot) input via throughfall and litterfall was estimated to 6.7 and 2.7 microg m(-2) yr(-1), respectively, which is considerably lower than previously reported from other boreal catchments in Scandinavia. A likely cause for the low input flux is the sparseness and low productivity of the forest in the Langtjern catchment, with less atmospheric scavenging and lower litterfall fluxes than previously studied sites. In addition there has been a general decrease in mercury (Hg) in the atmosphere on the northern hemisphere in the last decade. The estimated output flux of Hg(tot) with surface water was 2.5 microg m(-2) yr(-1), which is comparable to what has been reported elsewhere. The ratio of Hg(tot) output flux to input flux was 26%, which is considerably higher than reported from other sites. This illustrates that catchment properties have greater importance for surface water export of Hg than the current atmospheric input. The estimated total soil pool of Hg(tot) in the catchment was 17.4 mg m(-2). This corresponds to roughly 8000 years of the current surface water output flux and 2000 years of the current input flux.